Quantifying the distinct role of plasmon enhancement mechanisms in prototypical antenna-reactor photocatalysts
Plasmonic photocatalysis enabled by the unique localized surface plasmon resonance represents a promising approach for efficient solar energy conversion. Elucidating the distinct plasmonic catalytic mechanisms and quantification of their effect is crucial yet highly challenging, due to their complex and synergistic nature. Herein, we achieve the differentiation and quantification of thermal as well as various non-thermal reaction mechanisms in prototypical Au-[Fe(bpy)<sub>3</sub>]<sup>2+</sup> antenna-reactor photocatalysts using water splitting as test reaction. Through modification of the resonance condition and connection schemes, non-thermal plasmonic charge and energy transfer mechanisms are selectively shielded. It is found that plasmonic charge carrier-induced photochemistry dominates the photocurrent (~57%) in a reducing, hydrogen evolution environment; whereas resonant plasmonic energy transfer dominates (~54%) in an oxidative, oxygen evolution environment. Our approach provides generalized and fundamental understandings on the role of surface plasmons in photocatalysis as well as important design principles for plasmonic photocatalysts towards distinct reaction types and catalyst configurations.
Authors
- Jiahui Shen
- Jiari He
- Bo Wu (ORCID: https://orcid.org/0000-0002-7177-9029)
- Zidi Wang
- Xudong Dong (ORCID: https://orcid.org/0000-0002-8339-5604)
- Alexander Genest (ORCID: https://orcid.org/0000-0003-3968-7156)
- Kaiqi Nie (ORCID: https://orcid.org/0000-0002-1150-8024)
- Kai Feng (ORCID: https://orcid.org/0000-0003-3697-6139)
- Xingda An (ORCID: https://orcid.org/0000-0002-7484-7410)
- Yuxuan Zhou (ORCID: https://orcid.org/0009-0003-6371-1969)
- Binhang Yan (ORCID: https://orcid.org/0000-0003-2833-8022)
- Le He (ORCID: https://orcid.org/0000-0002-4520-0482)
- Zhiyi Wu (ORCID: https://orcid.org/0000-0002-3215-0092)
- Günther Rupprechter (ORCID: https://orcid.org/0000-0002-8040-1677)
- Shuang Liu (ORCID: https://orcid.org/0000-0002-9179-0065)
- Xiaohong Zhang (ORCID: https://orcid.org/0000-0002-6732-2499)
- Jiaqi Wang (ORCID: https://orcid.org/0000-0002-8806-8370)
- Binbin Zhang (ORCID: https://orcid.org/0000-0003-0839-0683)
- Zhijie Zhu
- Qingfeng Zhang (ORCID: https://orcid.org/0000-0002-7004-9040)
- Chaoran Li (ORCID: https://orcid.org/0000-0001-9517-8431)
- Ji Yu (ORCID: https://orcid.org/0000-0003-0775-8378)
- Xinge Hu
- Xiong Huang
- Yueru Ma
Institutions
- TU Wien (AT)
- Shandong University (CN)
- South China Normal University (CN)
- Wuhan University (CN)
- Soochow University (CN)
- Tsinghua University (CN)
Publication Details
- Journal
- Nature Communications
- Published
- 2025-03-06
- DOI
- https://doi.org/10.1038/s41467-025-57569-0
- Citations
- 46
- Primary Topic
- Advanced Photocatalysis Techniques
- Type
- article
- Field-Weighted Citation Impact
- 16.72
Funders
- National Natural Science Foundation of China